The aim of this study was to examine psychosocial and environmental predictors of cycling for transportation. A sample of 343 Flemish adults (43% men) living at maximum 10 km from their workplace was surveyed. Self-report measures of cycling, demographic variables, psychosocial variables, self-efficacy, perceived benefits and barriers and environmental attributes (destination, traffic variables and facilities at the workplace) of cycling for transport were obtained by means of a mailing questionnaire. Modeling and social support by accompanying, external self-efficacy, ecological-economic awareness and lack of time and interest were positively associated with the likelihood of cycling for transport and varied in importance between cyclists and non-cyclists. Cyclists estimate the time to destination shorter than non-cyclists and indicate to have more facilities for cyclists at the workplace. The results suggest that when people live in a setting with adequate bicycle infrastructure, individual determinants (psychosocial, self-efficacy, perceived benefits and barriers) outperform the role of environmental determinants in this sample. Promotion campaigns aimed at increasing cycling for transportation should focus on creating social support by encouraging cycling with partners, increasing self-efficacy, raising ecological and economic awareness, decreasing lack of time and interest barriers and providing facilities for cyclists at the workplace.